Innovation: Interfacial rheological properties of complex fluid-fluid interfaces are strongly influenced by the film microstructure. Experimental investigations for correlating interfacial morphology and rheology are notoriously challenging. A miniaturized radial Langmuir trough was developed to study complex fluid-fluid interfaces under purely dilatational deformations that operates in tandem with a conventional inverted microscope for simultaneous interfacial visualization. Experiments: Two materials were investigated at an air-water interface: poly(tert-butyl methacrylate) (PtBMA) and dipalmitoylphosphatidylcholine (DPPC). Surface pressure measurements made in the radial Langmuir trough were compared with a commercial rectangular Langmuir trough. Interfacial in situ visualization for each material was performed during the compression cycle in the radial trough. Challenges associated with the small size of the radial Langmuir trough, such as the influence of capillary deformation on the measured surface pressure, are also quantified. Findings: Measured surface pressures between the newly developed radial trough and the rectangular Langmuir trough compare well. Micrographs obtained in the radial Langmuir trough were used to obtain film properties such as Young's modulus. The new advance in colloid and interface science is the ability to capture structure-property relationships of planar interfaces using microscopy and purely dilatational deformation. This will advance the development of constitutive modeling of complex fluid-fluid interfaces. (c) 2020 Elsevier Inc. All rights reserved.